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同晶取代法制备Cu-Ni双金属催化剂及其催化CO加氢合成乙醇性能
引用本文:郑华艳,章敏,付华,张华成,李忠.同晶取代法制备Cu-Ni双金属催化剂及其催化CO加氢合成乙醇性能[J].燃料化学学报,2019,47(1):84-91.
作者姓名:郑华艳  章敏  付华  张华成  李忠
作者单位:Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
基金项目:国家自然科学基金(21576179,U1510203)资助
摘    要:采用定向同晶取代法制备了一系列镍孔雀石前驱体的Cu-Ni双金属催化剂。考察了前驱体结构以及催化剂表面组成对催化剂催化性能的影响,并采用浆态床反应器对催化剂的CO加氢制乙醇性能进行评价。实验结果表明,采用定向同晶取代法可以制备出(Cu,Ni)2CO3(OH)2纯物相,取代后的Ni2+主要富集在前驱体(Cu,Ni)2CO3(OH)2表面。焙烧后形成的(Cux,Ni1-x)O固溶体均匀地分散在CuO晶体结构中。还原后的催化剂中Cu、Ni相互均匀分散形成活性界面,促进了低碳醇的合成。其中,不连续分布的Ni活性位点阻止了碳链的进一步增长,从而提高了乙醇选择性。当Ni/Cu原料比为45:100时,(Cux,Ni1-x)O固溶体与CuO之间有较强的相互作用,表现出最好的反应活性和乙醇选择性。

关 键 词:合成气  乙醇  定向同晶取代  孔雀石结构  Cu-Ni催化剂  
收稿时间:2018-09-18

CO hydrogenation to ethanol over copper-nickel bimetallic catalyst prepared by isomorphous substitution method
ZHENG Hua-yan,ZHANG Min,FU Hua,ZHANG Hua-cheng,LI Zhong.CO hydrogenation to ethanol over copper-nickel bimetallic catalyst prepared by isomorphous substitution method[J].Journal of Fuel Chemistry and Technology,2019,47(1):84-91.
Authors:ZHENG Hua-yan  ZHANG Min  FU Hua  ZHANG Hua-cheng  LI Zhong
Abstract:A series of Cu-Ni bimetallic catalysts derived from nickel-malachite were prepared by an oriented isomorphous substitution method. The effects of the precursor structure and catalysts surface composition on the catalytic performance CO hydrogenation to ethanol were investigated in an agitated slurry autoclave reactor. The studies demonstrated that the pure (Cu,Ni)2CO3(OH)2 phase was obtained by oriented isomorphous substitution method and Ni2+ was rich on the (Cu,Ni)2CO3(OH)2 precursor surface. Uniform distribution of (Cux,Ni1-x)O solid solution were found in CuO crystal lattice. After calcination, the (Cux,Ni1-x)O solid solution dispersed in the crystal structure of CuO uniformly. Cu and Ni dispersed in the catalysts evenly to form an active interface after reduction, which promoted the synthesis of higher alcohols. Discontinuously distributed Ni-active sites prevented the carbon chain from growing further, and enhanced the selectivity of ethanol. The catalyst prepared by the feeding materials with Ni/Cu molar ratio=45:100 was found to exhibit higher activity and ethanol selectivity due to the strong interaction between (Cux,Ni1-x)O solid solution and CuO phase.
Keywords:syngas  ethanol  oriented isomorphous substitution method  malachite structure  Cu-Ni catalyst  
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